Abstract
This Roadmap article provides a succinct, comprehensive overview of the state of electronic structure (ES) methods and software for molecular and materials simulations. Seventeen distinct sections collect insights by 51 leading scientists in the field. Each contribution addresses the status of a particular area, as well as current challenges and anticipated future advances, with a particular eye towards software related aspects and providing key references for further reading. Foundational sections cover density functional theory and its implementation in real-world simulation frameworks, Green’s function based many-body perturbation theory, wave-function based and stochastic ES approaches, relativistic effects and semiempirical ES theory approaches. Subsequent sections cover nuclear quantum effects, real-time propagation of the ES, challenges for computational spectroscopy simulations, and exploration of complex potential energy surfaces. The final sections summarize practical aspects, including computational workflows for complex simulation tasks, the impact of current and future high-performance computing architectures, software engineering practices, education and training to maintain and broaden the community, as well as the status of and needs for ES based modeling from the vantage point of industry environments. Overall, the field of ES software and method development continues to unlock immense opportunities for future scientific discovery, based on the growing ability of computations to reveal complex phenomena, processes and properties that are determined by the make-up of matter at the atomic scale, with high precision.
| Original language | English |
|---|---|
| Article number | 042501 |
| Journal | Electronic Structure |
| Volume | 6 |
| Issue number | 4 |
| DOIs | |
| State | Published - Dec 1 2024 |
Funding
WAdJ acknowledges support from the Exascale Computing Project (17-SC-20-SC), a collaborative effort of the U.S. Department of Energy Office of Science and the National Nuclear Security Administration. JA Nash acknowledges support from The Molecular Sciences Software Institute, funded by the National Science Foundation under Grant CHE-2136142. PG and LG acknowledge support by the EU through the MaX Centre of Excellence for HPC applications (Project No. 101093378). DWY acknowledges support from the Exascale Computing Project (17-SC-20-SC), a collaborative effort of the U.S. Department of Energy Office of Science and the National Nuclear Security Administration. AJ acknowledges funding by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05-CH11231: Materials Project Program KC23MP. AHL acknowledges funding from the European Union\u2019s Horizon 2020 research and innovation program Grant Agreement No. 951786 (NOMAD CoE). GP acknowledges the NCCR MARVEL (a National Centre of Competence in Research, funded by the Swiss National Science Foundation, Grant No. 205602) and the European Union\u2019s Horizon 2020 research and innovation programme under Grant Agreement No. 957189 (BIG-MAP), also part of the BATTERY 2030+ initiative under Grant Agreement No. 957213. NG is supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through FWP 72684 at the Pacific Northwest National Laboratory (PNNL). YK is supported by the National Science Foundation under Award Nos. CHE-1954894 and OAC-2209858. XL is supported by the National Science Foundation under Award No. CHE-2154346 for the real-time ES theory development, and by the Department of Energy, Office of Science, Basic Energy Sciences, in the Heavy-Element Chemistry program for the development of the four-component Dirac framework (Grant No. DE-SC0021100) and the development of quantum field method (Grant No. DE-SC0006863). Open-source software development is supported by the National Science Foundation (OAC-2103717 to XL) and the Offices of Advanced Scientific Computing Research (ASCR) and Basic Energy Sciences (BES) of the U.S. Department of Energy (DE-SC0022263 to XL). PNNL is operated by Battelle Memorial Institute for the United States Department of Energy under DOE Contract No. DE-AC05-76RL1830. This material is based upon work supported by the National Science Foundation under Awards CHE-1954348 (to SHS) and CHE-1955302 (to NM). MR acknowledges funding from the Max Planck Society and the Deutsche Forschungsgemeinschaft (DFG)\u2014Projektnummer 182087777\u2014SFB 951. JEM and the Molecular Sciences Software Institute are supported by NSF Grant No. CHE-2136142. CB acknowledges funding from the Ministry of Culture and Science of the German State of North Rhine-Westphalia (MKW) via the NRW-R\u00FCckkehrprogramm. This work used computational resources of the supercomputer Fugaku provided by RIKEN through the HPCI System Research Project (Project ID: hp200179), and was supported by MEXT as \u2018Program for Promoting Research on the Supercomputer Fugaku\u2019 (Realization of innovative light energy conversion materials utilizing the supercomputer Fugaku, Grant Number JPMXP1020210317). TDC is supported by the U.S. National Science Foundation via Grants CHE-2154753 and CHE-2136142. CD appreciates support from the European Union\u2019s Horizon 2020 research and innovation program under the Grant Agreement No. 951786 (NOMAD CoE) and from the Deutsche Forschungsgemeinschaft (DFG), Project 182087777 (SFB 951). JA acknowledges support from the National Science Foundation, Grant CHE-2152633. TLW acknowledges support from the Exascale Computing Project (17-SC-20-SC), a collaborative effort of the U.S. Department of Energy Office of Science and the National Nuclear Security Administration, and by the U. S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Division of Chemical Sciences, Biological Sciences, and Geosciences Division at the Ames National Laboratory, which is operated by Iowa State University under Contract No. DE-AC02-07CH11358. VB acknowledges support by the National Science Foundation (NSF) under Award No. 1450280. Any opinions, findings, and conclusions or recommendations expressed here are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. SM thanks the Japanese Science and Technology Agency for financial support (Grant JST-ERATO JPMJER1903) and HBS thanks the National Science Foundation US for funding (Grant CHE1856437). L A B was supported in part by the U.S. National Science Foundation through Grant ACI-1449723. M J T O wishes to thank CECAM for its continuing support of the Electronic Structure Library initiative and all the people who have contribute to the project since its inception. L V S acknowledges support of the U.S. National Science Foundation (Grants CHE-1800505, CHE-2102639). SL thanks the Academy of Finland for financial support under Project Numbers 350282 and 353749. GB and SB acknowledge financial support from the MaX Center of Excellence funded by the EU through the H2020-INFRAEDI-2018 (Project: GA 824143). The authors would like to thank Michiel J van Setten, Kiroubanand Sankaran, Sergiu Clima for their contributions and the Imec Industrial Affiliation Program (IIAP) for funding. The work was also partially supported by the JSPS Grant-in-Aid for Transformative Research Areas (A) (21H05560 and 23H04105).
Keywords
- electronic structure
- future directions
- software